3.1. Conventional Transmission Line Method
Before applying our two-step fitting approach (TSFA), we analyze the data measured on the bottom-contact DNTT TFTs using the popular transmission line method (TLM). This analysis is performed to (i) put the measured current-voltage characteristics into a perspective commonly shared in our field of research and (ii) highlight the benefits and drawbacks of the conventional TLM.
In principle, the TLM can also handle certain non-idealities, such as non-Ohmic contact resistances. However, when applying the most commonly-used extraction procedure proposed in the conventional TLM, the model assumptions are rather strict and require (i) an ideal field-effect transistor in the gradual channel approximation [
23] having a charge-carrier mobility that is independent of the electric fields and the charge-carrier density and (ii) Ohmic source and drain resistances [
14,
15]. Under these model assumptions, the drain current
in the linear regime of the output characteristics is implicitly determined by:
The transfer length
accounts for a channel-length-independent extension of the charge-accumulation channel at the contacts. In bottom-gate, top-contact TFTs,
can be interpreted as an additional distance that the charge carriers travel laterally through the organic semiconductor layer underneath the contacts to reach the charge-accumulation channel (or the drain contact) (see, e.g., [
18]). In bottom-gate, bottom-contact TFTs, charges are injected and extracted very close to the channel, so the distances that the carriers travel above the contacts before reaching the channel (or the drain) are very small. This implies that in bottom-gate, bottom-contact TFTs,
is not necessarily a physically-interpretable parameter, but rather has to be seen as a weighting factor for a non-Ohmic contribution to the contact resistance.
The parameter extraction procedure consists of three parts. In the first part, the on-state resistance
is calculated from the slope of the measured output characteristics:
with
. Note that it is important to extract
for
V because only at this point is it possible to separate the contacts clearly from the channel within the model (cf.
Figure S1 in the Supplementary Materials). To determine
, we performed a linear fit to the output curves measured for the four smallest drain-source voltages and forced this fit to pass through the origin at
V and
A. The plot of the on-state resistance
as a function of the channel length
L for different gate-source voltages is shown in
Figure 2a. As can be seen, the measured on-state resistance is indeed proportional to the channel length, and the linear fits to the measured on-state resistance at different gate-source voltages intersect approximately at
m and
k
cm.
In the second part of the TLM analysis, the inverse slope
is extracted from
Figure 2a and plotted as a function of the gate-source voltage
(see
Figure 2b). The slope of this plot yields the intrinsic channel mobility
cm
/Vs, and the x-axis intersect yields the threshold voltage
V. In the last part of the TLM analysis, the on-state resistance at a channel length of zero,
, is plotted as a function of the sheet resistance
(see
Figure 2c). The slope of the linear fit to this data is the transfer length
m, and the y-axis intersect yields the Ohmic contact resistance
k
cm.
The parameters extracted from the conventional TLM analysis can be considered to be reliable only if the following requirements are fulfilled:
The measured output characteristics (gray symbols in
Figure 3a–d) must be linear for very small drain-source voltages (
V), and the slope of the curves must decrease monotonically as the absolute value of the drain-source voltage
increases. An S-shape of the output curves in this regime is an indicator of a non-Ohmic contact resistance.
The relations
versus
L (
Figure 2a),
versus
(
Figure 2b), and
versus
(
Figure 2c) must be linear.
The values for the transfer length
and the total Ohmic contact resistance
obtained from the plot
versus
(
Figure 2c) must be equal to the values for
L and
at the intersection in
Figure 2a.
Figure 2 and
Figure 3 confirm that all of these requirements are indeed fulfilled for our set of bottom-gate, bottom-contact DNTT TFTs. Small deviations of the on-state resistances
extracted for different channel lengths from the linear fit (see
Figure 2a) can be attributed to device-to-device variations. A closer look, however, reveals other, more serious inconsistencies. The inset in
Figure 2a shows a close-up of the
versus
L relation close to
together with the on-state resistances
for the smallest channel length
m (symbols). As can be seen, the linear fits to the
versus
L data do not intersect in a single point. In addition, all the on-state resistances
extracted from the data of the TFT with the smallest channel length (
m) are a factor of approximately two below the corresponding linear fits. These two inconsistencies do not invalidate a further analysis, because the fact that the linear fits to the
versus
L data do not intersect in a single point could just be a consequence of the drain-source voltage
being too large to be able to extract the on-state resistance
in a reliable manner (cf.
Figure S1), and the deviation of the on-state resistances
extracted from the data of the TFT with the channel length of
m might be caused by short-channel effects. These explanations do not necessarily compromise the validity of the model system.
As we are able to calculate the electrical TFT characteristics for a given set of device parameters, we can now compare the output and transfer characteristics calculated using the parameters extracted from the TLM analysis to the measured output and transfer characteristics. This comparison is shown in
Figure 3a–h for TFTs with channel lengths of 2, 8, 40, and 80
m. As can be seen, the calculated output curves (black lines) deviate substantially from the measured output curves (gray symbols), regardless of the channel length. These deviations indicate a problem within the transistor model underlying the TLM that had evaded the reliability check performed above. Upon closer inspection, it can be noticed that the agreement between the calculated and measured output and transfer curves is particularly poor when the channel length is small (
Figure 3a,e). For the three larger channel lengths (8, 40, and 80
m;
Figure 3b–d), the slope of the output curves at small drain-source voltages (linear regime) is captured reasonably well, but the agreement becomes increasingly worse with increasing absolute value of the drain-source voltage (saturation regime). The better agreement between the calculated and the measured output curves at small drain-source voltages (linear regime) is due to the fact that the transistor parameters in the TLM analysis were extracted for
V.
3.2. TSFA with Constant-Mobility Model
The conventional TLM analysis is able to produce reliable results only if all model parameters are identical for all transistors within the set of devices with different channel lengths. This is a substantial weakness of the conventional TLM, because in reality, these parameters can vary considerably, even for nominally identical organic transistors. Such device-to-device variations may explain the deviations between the calculated and the measured output and transfer characteristics, as seen in
Figure 3a–h. Therefore, the question arises whether these deviations can be attributed to the extraction method (TLM) or to the underlying transistor model. To answer this question, we have analyzed the measured TFT data using our TSFA. We have extracted a charge-carrier mobility
, a threshold voltage
, and source and drain resistances
and
for each TFT individually. Note that the transfer length
cannot be evaluated in the first step of the TSFA, and the charge-carrier mobility extracted within the TSFA is related to the intrinsic channel mobility
extracted using the TLM as
. The output and transfer characteristics calculated with this approach are shown in
Figure 3i–p. For all channel lengths, the agreement between the output and transfer curves calculated using our TSFA and the measured output and transfer curves (
Figure 3i–p) is significantly better than the agreement between the output and transfer curves calculated using the parameters obtained from the conventional TLM analysis and the measured output and transfer curves (
Figure 3a–h). The deviations between the calculated and the measured output characteristics seen in
Figure 3i–l are discussed in detail below. Since these deviations are relatively small and the deviations in the transfer curves (
Figure 3m–p) are even smaller, the main message taken from
Figure 3i–p is that the first step of our TSFA is conditionally passed.
For the second step of our TSFA, we plot the extracted transistor parameters as a function of the channel length, as shown in
Figure 4. To be consistent with the model assumptions, these parameters would have to be independent of the channel length
L.
Figure 4 shows that this is clearly not the case. In
Figure 4a, it can be seen that the absolute value of the threshold voltage
decreases by about 100 mV as the channel length is decreased from 40
m–2
m. This is the well-known threshold-voltage roll-off that occurs in all field-effect transistors (cf. [
30], Chapter 6.4.2).
Figure 4b shows a pronounced dependence of the charge-carrier mobility
on the channel length
L (symbols). If we were to strictly stick to the model underlying the TLM, we could surmise that this dependence might be related to the transfer length
. To check whether the introduction of a transfer length conceptually lifts the observed channel-length dependence, we can incorporate
into the second step of the TSFA by replacing the mobility
with the term
, where
should be independent of the channel length. This relation is reminiscent of, but not equivalent to the relation between effective mobility and intrinsic channel mobility (cf. [
21,
31]). A fit to the relation
is shown as a solid line in
Figure 4b. As can be seen, the agreement between the fit and the data is quite poor, as the fit systematically overestimates the extracted parameters for intermediate channel lengths (
m) and underestimates them for large channel lengths (
m). This poor agreement indicates a problem with the model system.
Figure 4c displays the combined contact resistance
. Rather than being independent of the channel length, the contact resistance
increases by more than a factor of three with increasing channel length, which is a clear indicator of an inadequate transistor model.
An explanation for the failure of the constant-mobility model can be found by taking a closer look at the deviations between the calculated and the measured output characteristics in
Figure 3i–l. We notice that neither the transition between the linear regime and the saturation regime, nor the saturation of the drain current at large drain-source voltages in the measured output curves are properly reproduced in the calculated output curves. The first of these symptoms occurs regardless of the channel length and can be alleviated by assuming that the charge-carrier mobility is a function of the charge-carrier density of the form
, as suggested by the percolation theory [
24] or by the multiple trapping and release model [
25]. The second symptom is more pronounced for shorter channels, which indicates a field-dependence of the charge-carrier mobility. As a first attempt, we assume a simplified Poole–Frenkel behavior of the form
[
7,
26].
3.3. TSFA with Field- and Charge-Carrier-Density-Dependent Mobility
Incorporating a field- and charge-carrier-density-dependent mobility in the model leads to a significantly better agreement between the calculated and the measured output and transfer characteristics (
Figure 5a–h) compared to the constant-mobility model (cf.
Figure 3i–p). Especially for the TFT with the smallest channel length (
Figure 3i,m and
Figure 5a,e), the agreement is substantially improved due to the fact that the Poole–Frenkel model provides a far more realistic description of the saturation regime. For all channel lengths, the agreement between the calculated and the measured output curves (
Figure 5a–d) is nearly perfect for the smaller gate-source voltages (
V). For the transfer curves (
Figure 5e–h), a slight improvement at the branching point at a gate-source voltage of about
V can be seen compared to the constant-mobility model (
Figure 3m–p). We again move on to examine the channel-length dependence of the extracted parameters. The most relevant parameters are the mobility prefactor
and the combined contact resistance
shown in
Figure 5i,j. The mobility prefactor
exhibits a slightly smaller channel-length dependence compared to the charge-carrier mobility
examined earlier (cf.
Figure 4b). The channel-length dependence of
is even more pronounced, with a ratio of approximately one order of magnitude between that of the TFT with the largest channel length and that of the TFT with the smallest channel length (see
Figure 5j), causing this model to fail. To illustrate the significant influence of the channel-length-dependence of the contact resistance,
Figure S2 shows the disagreement between the calculated and the measured output characteristics when considering the contact resistances of the TFTs with the smallest channel length (
Figure S2a–d) and of the TFTs with the largest channel length (
Figure S2e–h). The remaining parameters,
,
, and
do not have such a pronounced channel-length dependence (not shown).
To identify the problem of the model, we again inspect the calculated and the measured output characteristics (
Figure 5a–d). For all channel lengths, the output curves calculated for
V lie above and the output curves calculated for
V lie below the measured output curves. This inaccurate spacing of the curves in the saturation regime is an indicator for a problem of the charge-carrier-density dependence of the charge-carrier mobility, which is predominantly determined by the gate-source voltage
. The spacing of the curves in the saturation regime is determined not only by the charge-carrier-density dependence of the mobility, but also by the contact resistances (explained in more detail in
Figure S3). Assuming a constant mobility and zero contact resistance, the saturation current
increases quadratically with the gate-source voltage,
. On the other hand, assuming a constant mobility and a very large contact resistance, the saturation current would increase linearly with increasing gate-source voltage. This means that increasing both the mobility and the contact resistance can lead to similar output curves for the largest gate-source voltage and different spacings for smaller gate-source voltages (see
Figure S3).
This effect may explain the increase of with L in the following way: If the charge-carrier- density dependence of the charge-carrier mobility is captured incorrectly, the spacing of the output characteristics for different gate-source voltages will be inaccurate, as well. The incorrect spacing can be compensated by a correspondingly incorrect choice of the contact resistances. As the error in the mobility scales with the channel length in the calculation of the drain current because it is a channel property and the influence of the contact resistance on the drain current is not affected by the channel length, the value extracted for the contact resistance is forced to scale with L in order to compensate the incorrect mobility.
The over- and under-estimation of the drain current for the second-most-negative and the most-negative gate-source voltage suggests that the contact resistance decreases the spacing for more-negative gate-source voltages and, hence, is too large. This change in spacing can alternatively be achieved if the mobility would decrease with increasing charge-carrier density. This decrease should occur only for large charge-carrier densities, because for small charge-carrier densities, i.e., at small gate-source voltages, the increasing mobility in the improved TFT model describes the measured output curves substantially better than the constant-mobility model. Thus, the evaluation of our TSFA suggests that the mobility should first increase and then decrease as the charge-carrier density is increased. Indications for such a behavior of the mobility were recently found experimentally by Bittle et al. [
32] and Uemura et al. [
33]; Fishchuk et al. [
34] suggested such a behavior from a theoretical point of view.
Besides improving the mobility, another possible problem with the transistor model is that the gradual channel approximation does not take into account that organic semiconductors are in principle electrical insulators and that all mobile charges have to be provided by the metal contacts. Unlike in field-effect transistors based on doped semiconductors, such as silicon MOSFETs, these mobile charges in organic semiconductors are not compensated in the semiconductor by charges of opposite polarity. This uncompensated charge accumulation affects the electric field at the source and drain contacts, and this effect becomes more pronounced with increasing channel length. Including this charge cloud in the transistor model might also help alleviate the channel-length dependence of the contact resistance.
3.4. Testing Other Organic-TFT Technologies
We note that the failure of the transistor model discussed above is not exclusive to the bottom-gate, bottom-contact DNTT TFTs investigated above, as the model has also failed for the bottom-gate, top-contact DNTT TFTs [
21] and the bottom-gate, bottom-contact pentacene and C
TFTs [
22]. For the bottom-gate, top-contact DNTT TFTs and the bottom-gate, bottom-contact C
TFTs, we were able to obtain acceptable agreement between the calculated and the measured current-voltage characteristics by modeling the non-linearity in the linear regime of the output characteristics using a gate-voltage-dependent Schottky diode at the source contact [
22]. Selected examples of calculated and measured output characteristics for each set of TFTs are shown in
Figure 6a–d. The deviations between the calculated output characteristics and the measured output characteristics are similar to those for the bottom-gate, bottom-contact DNTT TFTs, exhibiting an overestimation of the absolute value of the drain current for the largest absolute value of the gate-source voltage and an underestimation for the smaller ones.
Figure 6e–h shows the Ohmic component of the combined contact resistance
as a function of the channel length
L for the bottom-gate, top-contact DNTT TFTs (
Figure 6e), the bottom-gate, bottom-contact pentacene TFTs with Au contacts functionalized with 2-phenylpyrimidine-5-thiol (BP0-down) (
Figure 6f), and the bottom-gate, bottom-contact C
TFTs with Au contacts functionalized with either 4-(2-mercaptophenyl)pyrimidine (BP0-up) or biphenyl-4-thiol (BP0) (
Figure 6g,h). The approximately linear dependence of
on the channel length causes a similar failure of the transistor model during the second step of our TSFA for each set of TFTs.